Nucleation and condensational growth to CCN sizes during a sustained pristine biogenic SOA event in a forested mountain valley

Pierce, Jeffrey R.; Leaitch, W. R.; Liggio, John; Westervelt, Daniel M.; Wainwright, C.; Abbatt, Jonathan P. D.; Ahlm, Lars; Al-Basheer, Watheq; Cziczo, D. J.; Hayden, K. L.; Lee, Alex K. Y.; Li, S.-M.; Russell, Lynn M.; Sjostedt, S. J.; Strawbridge, K. B.; Travis, Michael S.; Vlasenko, A.; Wentzell, Jeremy J. B.; Wiebe, H. A.; Wong, J. P. S.; Macdonald, A. M.

doi:10.5194/acp-12-3147-2012

Cited by 132 publications

(138 citation statements)

References 55 publications

(76 reference statements)

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“…In the NH, prolonged pristine periods generally occur only over continental regions above 60°N, such as in boreal Canada (32) and Russia (33), where aerosol is affected strongly by natural forest fire emissions. Here, CCN concentrations are highly variable, but generally range from 100 to 1,000 cm −3 .…”

Section: Resultsmentioning

confidence: 99%

Occurrence of pristine aerosol environments on a polluted planet

Hamilton

Lee

Pringle

et al. 2014

Proc. Natl. Acad. Sci. U.S.A.

162

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Significance Uncertainty in aerosol forcing of climate since the preindustrial era hampers efforts to quantify the sensitivity of global temperature to radiative perturbations caused by human activity. Because forcings are referenced to preindustrial conditions, a large part of the uncertainty will be reduced only by accurately defining pristine aerosol conditions before air pollution. We show that pristine conditions should still be observable on a few days per month in many regions of the Earth. However, pristine cloudy regions, which are of most importance for forcing uncertainty, occur almost entirely in the Southern Hemisphere. Reduction in uncertainty of predominantly Northern Hemisphere forcing may therefore have to rely on measurements from a different hemisphere, which will limit the extent to which uncertainties can be reduced.

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Section: Resultsmentioning

confidence: 99%

Occurrence of pristine aerosol environments on a polluted planet

Hamilton

Lee

Pringle

et al. 2014

Proc. Natl. Acad. Sci. U.S.A.

162

172

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“…Ambient and laboratory studies have shown that sulfuric acid participates in the first steps of new particle formation (Weber et al, 1996;Sihto et al, 2006;Riipinen et al, 2007;Kuang et al, 2008;Sipilä et al, 2010;Vehkamäki and Riipinen, 2012;Kulmala et al, 2013), but sulfuric acid condensation is not enough to reproduce particle growth rates observed in the ambient conditions (Kuang et al, 2010;Sipilä et al, 2010;Pierce et al, 2011Pierce et al, , 2012Riipinen et al, 2011Riipinen et al, , 2012Kulmala et al, 2013). Therefore other compounds, e.g., organics or ammonia/amines, are expected to be important in the early growth of freshly nucleated particles (O'Dowd et al, 2002;Smith et al, 2005Smith et al, , 2008Pierce et al, 2011;Riipinen et al, 2012;Vehkamäki and Riipinen, 2012;Kulmala et al, 2013).…”

Section: S a K Häkkinen Et Al: Semi-empirical Parameterization Ofmentioning

confidence: 99%

Semi-empirical parameterization of size-dependent atmospheric nanoparticle growth in continental environments

et al. 2013

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The capability to accurately yet efficiently represent atmospheric nanoparticle growth by biogenic and anthropogenic secondary organics is a challenge for current atmospheric large-scale models. It is, however, crucial to predict nanoparticle growth accurately in order to reliably estimate the atmospheric cloud condensation nuclei (CCN) concentrations. In this work we introduce a simple semi-empirical parameterization for sub-20 nm particle growth that distributes secondary organics to the nanoparticles according to their size and is therefore able to reproduce particle growth observed in the atmosphere. The parameterization includes particle growth by sulfuric acid, secondary organics from monoterpene oxidation (SORG_MT) and an additional condensable vapor of non-monoterpene organics ("background"). The performance of the proposed parameterization was investigated using ambient data on particle growth rates in three diameter ranges (1.5–3 nm, 3–7 nm and 7–20 nm). The growth rate data were acquired from particle/air ion number size distribution measurements at six continental sites over Europe. The longest time series of 7 yr (2003–2009) was obtained from a boreal forest site in Hyytiälä, Finland, while about one year of data (2008–2009) was used for the other stations. The extensive ambient measurements made it possible to test how well the parameterization captures the seasonal cycle observed in sub-20 nm particle growth and to determine the weighing factors for distributing the SORG_MT for different sized particles as well as the background mass flux (concentration). Besides the monoterpene oxidation products, background organics with a concentration comparable to SORG_MT, around 6 × 10⁷ cm⁻³ (consistent with an additional global SOA yield of 100 Tg yr⁻¹) was needed to reproduce the observed nanoparticle growth. Simulations with global models suggest that the "background" could be linked to secondary biogenic organics that are formed in the presence of anthropogenic pollution

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“…Organic compounds are known to aid in the growth of newly formed particles (∼ 1-2 nm diameter) to observable sizes (> 3 nm diameter; Boy et al, 2003;Kulmala et al, 2004;Verheggen et al, 2007;Laaksonen et al, 2008;Pierce et al, 2011;Yli-Juuti et al, 2011;Riccobono et al, 2012) and even further to a CCN-active size (> ∼ 70 nm diameter; Riipinen et al, 2011Riipinen et al, , 2012Pierce et al, 2012;Paasonen et al, 2013). Additionally, the oxidation products of terpenes may play a role in the initial stages of particle formation via stabilisation of the critical nucleus (Fan et al, 2006;Zhang et al, 2009;Metzger et al, 2010;Paasonen et al, 2010;Kulmala et al, 2013).…”

Section: Introductionmentioning

confidence: 99%

The direct and indirect radiative effects of biogenic secondary organic aerosol

et al. 2014

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Abstract. We use a global aerosol microphysics model in combination with an offline radiative transfer model to quantify the radiative effect of biogenic secondary organic aerosol (SOA) in the present-day atmosphere. Through its role in particle growth and ageing, the presence of biogenic SOA increases the global annual mean concentration of cloud condensation nuclei (CCN; at 0.2 % supersaturation) by 3.6-21.1 %, depending upon the yield of SOA production from biogenic volatile organic compounds (BVOCs), and the nature and treatment of concurrent primary carbonaceous emissions. This increase in CCN causes a rise in global annual mean cloud droplet number concentration (CDNC) of 1.9-5.2 %, and a global mean first aerosol indirect effect (AIE) of between +0.01 W m −2 and −0.12 W m −2 . The radiative impact of biogenic SOA is far greater when biogenic oxidation products also contribute to the very early stages of new particle formation; using two organically mediated mechanisms for new particle formation, we simulate global annual mean first AIEs of −0.22 W m −2 and −0.77 W m −2 . The inclusion of biogenic SOA substantially improves the simulated seasonal cycle in the concentration of CCN-sized particles observed at three forested sites. The best correlation is found when the organically mediated nucleation mechanisms are applied, suggesting that the first AIE of biogenic SOA could be as large as −0.77 W m −2 . The radiative impact of SOA is sensitive to the presence of anthropogenic emissions. Lower background aerosol concentrations simulated with anthropogenic emissions from 1750 give rise to a greater fractional CCN increase and a more substantial first AIE from biogenic SOA. Consequently, the anthropogenic indirect radiative forcing between 1750 and the present day is sensitive to assumptions about the amount and role of biogenic SOA. We also calculate an annual global mean direct radiative effect of between −0.08 W m −2 and −0.78 W m −2 in the present day, with uncertainty in the amount of SOA produced from the oxidation of BVOCs accounting for most of this range.

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Nucleation and condensational growth to CCN sizes during a sustained pristine biogenic SOA event in a forested mountain valley

Cited by 132 publications

References 55 publications

Occurrence of pristine aerosol environments on a polluted planet

Occurrence of pristine aerosol environments on a polluted planet

Semi-empirical parameterization of size-dependent atmospheric nanoparticle growth in continental environments

The direct and indirect radiative effects of biogenic secondary organic aerosol

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